Journal
JOURNAL OF SOLID STATE CHEMISTRY
Volume 261, Issue -, Pages 92-102Publisher
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jssc.2018.02.016
Keywords
Gold nanoparticle; Titanium silicalite-1; Homogeneous deposition; Propylene epoxidation; Structure-reactivity relationship
Funding
- Fundamental Research Funds for the Central Universities of China [3207045403, 3207045409, 3207046414]
- National Natural Science Foundation of China [21576050, 51602052]
- Jiangsu Provincial Natural Science Foundation of China [BK20150604]
- Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)
- Southeast University
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We report a simple and efficient method for the preparation of highly dispersed Au nanoparticles (< 5 nm) on TS-1 substrate. The synthesis relies on the use of NaBH4 as a reductant for rapid Au atom generation, as well as PVA as a capping agent confining the particle size and dispersion. The samples were characterized by N-2 physisorption, inductively coupled plasma mass spectrometry, power X-ray diffraction, scanning electron microscopy, transmission electron microscopy, energy-dispersive X-ray spectroscopy, X-ray photoelectron spectroscopy, CO pulse chemisorption and thermogravimetric analysis. The size of Au particles can be controlled in the range of 3-5 nm. The supported catalyst shows both good activity and selectivity for propylene oxide (PO) generation from direct propylene epoxidation. An optimal performance with PO formation rate of 102.94 gpo h(-1) kg(-1) eat and selectivity of 84.83% is achieved over 2.0 wt% Au/TS-1 catalyst, which is prepared by controlling PVA/Au3+' mass ratio of 1.5/1 and NaBH4/Au3+ mole ratio of 5/1. After 50 h test at 200 degrees C, no significant decrement of both catalytic activity and PO selectivity can be observed, indicating the excellent thermally stability of the catalyst. Furthermore, a possible reaction mechanism is described on basis of the previous researches and our experimental results.
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